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超小纳米集群加速质子化,以获得高效的CO2电解向CO2的电解

Jun Wu^1,2, Wuyi Zhang¹, Lin Wu¹

¹School of Metallurgy and Environment, Central South University, Changsha, 410083, China.

Angewandte Chemie (International ed. in English)

|November 3, 2025

概括

超小纳米集群 (Ni3─N─C) 通过增强质子合电子转移来加速电化学CO2减排. 这种催化剂设计显著提高了二氧化碳的选择性,为高效的二氧化碳转化提供了一个有前途的战略.

科学领域:

电化学电化学电化学
材料科学材料科学材料科学
催化剂是一种催化剂.

背景情况:

质子合电子转移 (PCET) 对于电化学二氧化碳减排 (CO2RR) 是至关重要的.
在PCET中,质子化步骤往往是动力瓶,限制了CO2RR效率.
调节催化剂微结构以加速质子化是改善二氧化碳对二氧化碳选择性的关键策略.

研究的目的:

为增强CO2RR开发超小的Ni纳米集聚催化剂 (Ni3─N─C).
研究亚纳米集群中独特的Ni协调环境对催化性能的影响.
阐明Ni3─N─C催化剂改善速度限制型质子化步骤的机制.

主要方法:

在H2大气下含有Ni的前体的一步热解以合成Ni3─N─C催化剂.
电化学表征以评估CO2RR性能,包括法拉第效率 (FECO) 和超电位.
密度函数理论 (DFT) 计算以了解反应机制和能量障碍.
在现场FTIR光谱测试以确认中间形成和反应途径.

主要成果:

Ni3─N─C催化剂在广泛的电位范围 (-0.6到-1.0V与RHE) 中提供了高于90%的CO法拉戴效率,在 -0.8V时达到高峰值95%左右.
DFT的计算显示,Ni3─N─C降低了*COOH形成的能量屏障,这是由于吸附配置的改变造成的.
在现场FTIR证实了Ni3─N─C表面的加速*COOH形成,验证了增强的质子化步骤.

结论:

超小的Ni子纳米集群 (Ni3─N─C) 有效调节PCET,加速CO2RR中的限制速率的质子化步骤.
在Ni3─N─C中独特的局部Ni协调环境对于增强CO2到CO的选择性至关重要.
这项工作建立了基于纳米集群的催化剂的合理设计原则,以实现高效的电化学二氧化碳减排.

关键词:

减少二氧化碳的减少协调环境的修改.子纳米集群中的子纳米集群.质子合电子的电子转移.一个原子的催化剂.

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